原位紫外-可见-近红外吸收光谱和催化反应

IF 51.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Max L. Bols, Jing Ma, Fatima Rammal, Dieter Plessers, Xuejiao Wu, Sara Navarro-Jaén, Alexander J. Heyer, Bert F. Sels*, Edward I. Solomon* and Robert A. Schoonheydt*, 
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引用次数: 0

摘要

本综述重点介绍催化过程中的原位紫外-可见-近红外吸收光谱。文中讨论了确定反应机制、动力学和结构特性的各种实验技术。停流技术、激光脉冲的使用以及实验扰动的使用被展示在酶催化、均相催化、异相催化和光催化的原位研究中。这些技术可以进入不同的时间尺度,适用于不同的反应体系和催化剂类型。在光催化方面,讨论了通过瞬态吸收进行飞秒和纳秒分辨率测量,以跟踪激发态。特别针对铜、铁交换沸石和金属酶,展示了用于结构表征的紫外-可见-近红外吸收光谱。这需要结合不同的光谱。磁圆二色性和共振拉曼光谱的结合尤其强大。可以跟踪各种载体上过渡金属催化剂的多种现象,包括氧化态变化、吸附、反应、载体相互作用、表面等离子体共振和带隙。对氧化态、氧空位和带隙的测量显示了异质催化剂,尤其是电催化催化剂的氧化态、氧空位和带隙。紫外-可见-近红外吸收受到宽吸收带的影响。尽管光谱错综复杂,先进的分析技术仍能跟踪酸性沸石上的焦化反应。紫外-可见-近红外吸收光谱在催化剂表征和机理研究方面的价值是显而易见的,但还可以进一步拓展。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

In Situ UV–Vis–NIR Absorption Spectroscopy and Catalysis

In Situ UV–Vis–NIR Absorption Spectroscopy and Catalysis

In Situ UV–Vis–NIR Absorption Spectroscopy and Catalysis

This review highlights in situ UV–vis–NIR range absorption spectroscopy in catalysis. A variety of experimental techniques identifying reaction mechanisms, kinetics, and structural properties are discussed. Stopped flow techniques, use of laser pulses, and use of experimental perturbations are demonstrated for in situ studies of enzymatic, homogeneous, heterogeneous, and photocatalysis. They access different time scales and are applicable to different reaction systems and catalyst types. In photocatalysis, femto- and nanosecond resolved measurements through transient absorption are discussed for tracking excited states. UV–vis–NIR absorption spectroscopies for structural characterization are demonstrated especially for Cu and Fe exchanged zeolites and metalloenzymes. This requires combining different spectroscopies. Combining magnetic circular dichroism and resonance Raman spectroscopy is especially powerful. A multitude of phenomena can be tracked on transition metal catalysts on various supports, including changes in oxidation state, adsorptions, reactions, support interactions, surface plasmon resonances, and band gaps. Measurements of oxidation states, oxygen vacancies, and band gaps are shown on heterogeneous catalysts, especially for electrocatalysis. UV–vis–NIR absorption is burdened by broad absorption bands. Advanced analysis techniques enable the tracking of coking reactions on acid zeolites despite convoluted spectra. The value of UV–vis–NIR absorption spectroscopy to catalyst characterization and mechanistic investigation is clear but could be expanded.

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来源期刊
Chemical Reviews
Chemical Reviews 化学-化学综合
CiteScore
106.00
自引率
1.10%
发文量
278
审稿时长
4.3 months
期刊介绍: Chemical Reviews is a highly regarded and highest-ranked journal covering the general topic of chemistry. Its mission is to provide comprehensive, authoritative, critical, and readable reviews of important recent research in organic, inorganic, physical, analytical, theoretical, and biological chemistry. Since 1985, Chemical Reviews has also published periodic thematic issues that focus on a single theme or direction of emerging research.
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